Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Publication date: 16th December 2024
Empirical A-site cation substitution has advanced the stability and efficiency of hybrid organic-inorganic lead halide perovskite solar cells and the functionality of X-ray detectors. Yet, the fundamental mechanisms underpinning their unique performance remain elusive. This multi-modal study unveils the link between nanoscale structural dynamics and macroscopic optoelectronic properties in these materials by utilising X-ray diffuse scattering, inelastic neutron spectroscopy and a suite of hyperspectral microscopy tools complemented by state-of-the-art machine learning-assisted molecular dynamics simulations. Our approach confirms the presence of dynamic, lower-symmetry local nanodomains embedded within the higher-symmetry average phase in various perovskite compositions. The properties of these nanodomains are tunable via the A-site cation selection: methylammonium induces a high density of anisotropic, planar nanodomains of out-of-phase octahedral tilts, while formamidinium favours sparsely distributed isotropic, spherical nanodomains with in-phase tilting, even when crystallography reveals cubic symmetry on average. We demonstrate that these sparsely distributed isotropic nanodomains reduce electronic dynamic disorder, resulting in a beneficial optoelectronic response, thereby enhancing the performance of lead halide perovskite devices. By demonstrating the influence of A-site cation on local nanodomains and consequently, on macroscopic properties, we propose leveraging this relationship to engineer the optoelectronic response of these materials, propelling further advancements in perovskite-based photovoltaics, optoelectronics, and X-ray imaging.
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